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Activation of urchin-like Ni-doped W18O49/NF by electrochemical tuning for efficient water splitting
Journal of Energy Chemistry ( IF 13.1 ) Pub Date : 2021-09-04 , DOI: 10.1016/j.jechem.2021.08.056
Guojuan Hai 1, 2 , Jianfeng Huang 1 , Liyun Cao 1 , Koji Kajiyoshi 3 , Long Wang 4 , Liangliang Feng 1, 3 , Jun Chen 2
Affiliation  

The electrochemical conversion is closely correlated with the electrocatalytic activities of the electrocatalyst. Herein, the urchin-like Ni-doped W18O49/NF with enriched active sites was prepared by solvothermal method followed by a low-temperature pyrolysis treatment was reported. Results demonstrate that the incorporation of Ni-doping triggers the lattice distortion of W18O49 for the increasement of oxygen defects. Further, high-valent W6+ are partially reduced to low-valent W4+, wherein the electrons originate from the oxidation process of Ni2+ to Ni3+. The Ni3+ ions show an enhanced orbital overlap with the OER reaction intermediates. The generated W4+ ions contribute to release oxygen vacancies, eventually reorganizing Ni-doped W18O49/NF to unique electrochemical active species with a special amorphous-crystalline interface (AM/NiWOx/NiOOH/NF). Simultaneously, the reconstruction results in an optimized valence band and conduction band. Eventually, the resultant AM/NiWOx/NiOOH/NF with abundant active sites and improved oxidation/reduction capability exhibits more superior catalytic performance compared with the Ni-doped W18O49/NF counterpart. This study gives more insights in the electrochemical evolution of the tungsten-based oxide and provides effective strategies for optimizing the catalytic activity of materials with inherent hydrogen evolution reaction limitations.



中文翻译:

通过电化学调谐激活类海胆的 Ni 掺杂 W18O49/NF 以实现高效的水分解

电化学转化与电催化剂的电催化活性密切相关。在此,报道了通过溶剂热法和低温热解处理制备了具有富集活性位点的类海胆状Ni掺杂W 18 O 49 /NF。结果表明,Ni 掺杂的掺入引发了 W 18 O 49的晶格畸变,从而增加了氧缺陷。此外,高价W 6+部分还原为低价W 4+,其中电子来自Ni 2+到Ni 3+的氧化过程。尼3+离子与 OER 反应中间体显示出增强的轨道重叠。生成的 W 4+离子有助于释放氧空位,最终将 Ni 掺杂的 W 18 O 49 /NF重组为具有特殊非晶-晶界面 (AM/NiWO x /NiOOH/NF) 的独特电化学活性物质。同时,重建导致优化的价带和导带。最终,与Ni掺杂的W 18 O 49相比,具有丰富活性位点和改进的氧化/还原能力的AM/NiWO x /NiOOH/NF表现出更优异的催化性能/NF 对应物。该研究为钨基氧化物的电化学演化提供了更多见解,并为优化具有固有析氢反应限制的材料的催化活性提供了有效策略。

更新日期:2021-09-04
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